A technological need exists to better prepare metal, polymer, ceramic, and glassy structures at the micro and nanoscale including preparation of patterned structures at high resolution and registration. For example, patterned polymeric structures have attracted significant interest for applications in the development of, for example, sensors, catalysis, and optical devices.[1,2] Thus far, several strategies, based upon photolithography, electron beam lithography, and micro-contact printing have been developed for generating polymer arrays.[2] While useful for some applications, these methods do not generally allow one to control nanostructure composition in a site-specific manner, and therefore, do not generally allow one to fabricate complex multi-component polymer arrays over the nano- to microscopic length scales. Having the capability to generate multi-component arrays with nanoscopic features would afford one the opportunity to construct and study high-density combinatorial libraries of novel macromolecular systems. A general need exists to be able to combine high registration, high resolution patterning with microscopic and nanoscopic control of polymerization, including formation of polymer brushes. Small structures prepared at high resolution and excellent registration, and with careful control of composition, are needed. A need also exists to better control reactions which can occur when a compound is deposited from a tip to a surface, particularly when the tip is a fine, nanoscopic, sharp tip.